tempo and pyrene

The work presented herein demonstrates a hybrid bi-catalytic architecture for the complete electrochemical oxidation of ethanol. The new catalytic system contains pyrene-TEMPO (TEMPO = 2,2,6,6-tetramethylpiperidinyl-N-oxyl) immobilized on the surface of carboxylated multi-walled carbon nanotubes (MWCNT-COOH), and oxalate decarboxylase enzyme (OxDc) immobilized onto a carbon cloth electrode. Electrolysis revealed a stable amperometric curve and an excellent current density value over a duration of 10 h. In addition, the hybrid system immobilized on the carbon electrode exhibits outstanding stability after electrolysis. Nuclear magnetic resonance (NMR) and gas chromatography (GC) demonstrate that the hybrid electrode system is able to oxidize ethanol to CO

Topics: Biosensing Techniques; Carbon Dioxide; Carboxy-Lyases; Catalysis; Cyclic N-Oxides; Electrolysis; Enzymes, Immobilized; Ethanol; Nanotubes, Carbon; Pyrenes

Electrocatalytic methods for organic synthesis could offer sustainable alternatives to traditional redox reactions, but strategies are needed to enhance the performance of molecular catalysts designed for this purpose. The synthesis of a pyrene-tethered TEMPO derivative (TEMPO=2,2,6,6-tetramethylpiperidinyl-N-oxyl) is described, which undergoes facile in situ noncovalent immobilization onto a carbon cloth electrode. Cyclic voltammetry and controlled potential electrolysis studies demonstrate that the immobilized catalyst exhibits much higher activity relative to 4-acetamido-TEMPO, an electronically similar homogeneous catalyst. In preparative electrolysis experiments with a series of alcohol substrates and the immobilized catalyst, turnover numbers and frequencies approach 2 000 and 4 000 h

Topics: Alcohols; Catalysis; Cyclic N-Oxides; Electrochemical Techniques; Molecular Structure; Oxidation-Reduction; Pyrenes